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pubs.acs.org/NanoLett
Laboratory of Thermodynamics in Emerging Technologies, Department of Mechanical and Process Engineering, ETH Zurich, 8092
Zurich, Switzerland
ABSTRACT: The great majority of investigations of thermal transport in carbon
nanotubes (CNTs) in the open literature focus on low heat uxes, that is, in the regime
of validity of the Fourier heat conduction law. In this paper, by performing
nonequilibrium molecular dynamics simulations we investigated thermal transport in a
single-walled CNT bridging two Si slabs under constant high heat ux. An anomalous
wave-like kinetic energy prole was observed, and a previously unexplored, wavedominated energy transport mechanism is identied for high heat uxes in CNTs,
originated from excited low frequency transverse acoustic waves. The transported energy,
in terms of a one-dimensional low frequency mechanical wave, is quantied as a function
of the total heat ux applied and is compared to the energy transported by traditional
Fourier heat conduction. The results show that the low frequency wave actually
overtakes traditional Fourier heat conduction and eciently transports the energy at high
heat ux. Our ndings reveal an important new mechanism for high heat ux energy
transport in low-dimensional nanostructures, such as one-dimensional (1-D) nanotubes
and nanowires, which could be very relevant to high heat ux dissipation such as in micro/nanoelectronics applications.
KEYWORDS: Low-frequency wave, high heat ux, energy transport, carbon nanotube, molecular dynamics
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Figure 1. (top) Schematic of a (5,5) single-walled CNT with 1600 unit cells (400 nm long) connected to Si slabs of 8 8 16 unit cells. Color
coding: cyan, C; yellow, Si. (bottom) Corresponding total kinetic energy, external energy, and real temperature distribution for the CNT. The real
temperature is calculated by only using the internal energy. The total kinetic energy and the external energy are normalized by 3/2NkB to facilitate
comparison with the real temperature. See denitions of these energies in the text.
actual reported data represent the steady state averages over the
last 0.5 ns of each production run.
A typical temperature prole of a (5,5) CNT under the high
heat ux of 464 GW/m2 is presented in the bottom panel of
Figure 1 (the range of heat ux values that can be termed
high will be discussed later in the paper). For the CNT crosssection area, we follow the standard practice of treating the
single-walled CNT as a hollow tube of diameter d and a wall
thickness of h = 3.4 .8,26 The diameter values are d = 6.9
and 13.8 for (5,5) and (10,10) CNT, respectively. This gives
the cross-section area of dh. Surprisingly, an anomalous wavelike overall temperature prole is observed (see black line in
Figure 1). Strictly speaking, this is the total kinetic energy
prole and not the real temperature prole of the CNT, as we
will explain later. We studied a video of the CNT motion in
VMD software27 and found that the CNT vibrates signicantly
in this case. The same wave-like overall temperature prole was
found in the (10,10) CNT for heat ux around 500 GW/m2.
We rst excluded the artifacts possibly induced by the Muller
Plathe method employed and conrmed our results by reducing
the heat ux to 16 and 122 GW/m2 for (5,5) and (10,10)
CNT, respectively. The simulation shows that as heat ux is
reduced no noticeable CNT vibration occurs and the overall
temperature prole of the CNT is practically linear on both
sides of the heat source region with two well-dened constant
temperature gradients (not shown for brevity), from which we
obtained the thermal conductivity of the (5,5) and (10,10)
CNTs to be 196 4 and 229 6 W/mK, respectively, in good
agreement with previous studies.2830 This underpins our
ndings of the wave-like overall temperature prole occurring
only at high heat uxes.
We analyze the anomalous temperature prole starting with
the velocities of atoms. We consider the CNT atoms in each
slice as an ensemble. For each slice we decompose the total
velocity of each CNT atom (tot) in the slice into a translational
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1
N
N
i
tot,
(1b)
i=1
Ektot =
i=1
N
Eext =
E int =
i=1
1
i
2
mi(tot,
)
2
(2a)
1
mi(tr i , )2
2
(2b)
3
NkBT =
2
i=1
1
i
2
mi(ran,
)
2
(2c)
(3a)
dx.doi.org/10.1021/nl300261r | Nano Lett. 2012, 12, 34103416
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PW =
1 2 2
A Vg
2
T
PF = 2 Ac
z
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(3b)
Vg =
(3c)
(4)
where Ptot is the total input heat power into the CNT,
determined by the input parameter of the MullerPlathe
method, PW and PF the heat power transported by the
mechanical wave and by Fourier conduction, respectively, the
mass of the CNT per unit length, the angular frequency, A
the wave amplitude, Vg the phonon group velocity, the
thermal conductivity of the CNT, T/z the real temperature
gradient along the tube axis, and Ac the cross-sectional area of
the CNT. The factor of 2 in eq 3c accounts for the Fourier heat
ow in the left and right directions. To obtain the phonon
group velocity Vg, we rst calculated the phonon dispersion
curves of the (5,5) and (10,10) CNTs using the PHONOPY
Figure 3. (top) Phonon dispersion curves of (5,5) (a) and (10,10) (b)
CNT. a is the lattice constant of the CNT in the axial direction, and k
is the wave vector. The thick red lines identify the two degenerated
transverse acoustic (TA) phonon modes. (bottom) Corresponding
phonon group velocity (low frequency part) of (5,5) (c) and (10,10)
(d) CNT as a function of frequency. Insets: full phonon group
velocity.
3413
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22 C 3T0 3
(5)
Figure 4. Frequency of the excited transverse acoustic wave in a 400nm-long CNT (a), percentage of wave-transported energy (b), and
thermal conductivity of CNT (c) as a function of the total heat ux. In
b, : the eciency of exciting the mechanical wave; : the maximum
eciency for a Carnot cycle; : two-thermostat method; : constant
heat ux method; : MullerPlathe method with REBO potential;
the black dashed line denotes the critical heat ux (qc) beyond which
CNT starts to vibrate signicantly; thus, the low frequency mechanical
wave dominates the energy transport.
wave
3414
Eext|wave
T
max
1 C Carnot
Q
TH
(6)
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AUTHOR INFORMATION
Corresponding Author
Notes
ACKNOWLEDGMENTS
X.Z. gratefully acknowledges the scholarship of the State
Scholarship Fund of the China Scholarship Council that
allowed him to be a visiting student at ETH Zurich and
contribute to this work. Computational support from the
Brutus Cluster at ETH Zurich and Supercomputing Center of
CAS in China is also gratefully acknowledged. This work was
supported by a grant from the Swiss National Supercomputing
Centre-CSCS under project ID s243 and s359.
REFERENCES